Poly(vinyl　alcohol)　(PVA)　aerogels　with　excellent　environmentally　friendly　properties　have　been　considered　to　replace　undegradable　polymer　foams.　However,　due　to　highly　flammable,　hydrophilic,　and　worse　compression　resistance　performance,　PVA　aerogels　have　always　been　excluded　from　practical.　Herein,　a　fire　safety　and　compression　resistance　PVA/expansible　graphene　oxide　(EGO)/Layered　double　hydroxides　(LDHs)　(PGL)　aerogel　was　prepared　via　the　freeze-drying　method　and　electrostatic　adsorption　of　flame　retardant.　The　ice　crystals　from　aerogels　were　sublimated　and　left　a　mass　of　tree-like　pore　tunnel　structures.　Meantime,　the　compound　of　EGO　and　LDHs　rendered　PGL　aerogels　high　compressive　strength　of　6.0917　MPa　(at　80%　of　strains),　a　high　specific　modulus　of　19.16　m2/s2,　and　an　ultra-low　density　of　0.059　g/cm3.　Especially,　the　as-prepared　PGL　aerogels　showed　heat　release　reduced　by　55.4%,　smoke　release　reduced　by　54.3%,　and　the　limiting　oxygen　index　reaching　up　to　31%.　Moreover,　LDHs　also　enhanced　the　interface　with　PVA/EGO　resulting　in　hydrophobic　performance　improvement.　The　proposed　enhancements　mechanism　suggested　that　(i)　chemical　reactions　between　EGO　and　PVA　matrix;　(ii)　a　mass　of　negative　potential　sites　from　the　interface　of　PVA/EGO　composites　made　LDHs　sheets　easily　adsorbing;　(iii)　oxygen-containing　groups　from　EGO　and　LDHs　absorbed　mass　of　heat　during　combustion;　(iv)　the　compact　char　residues　on　the　surface　of　aerogels　acting　as　barriers　suppressed　smoke　and　prevented　PVA　matrix　from　further　combustion.　Therefore,　electrostatic　adsorption　as　a　facile　production　process　was　paved　for　meeting　the　compression　resistance,　flame-retardant,　heat-insulating,　and　smoke-suppressed　requirements　of　PVA　aerogels　in　this　work.　©　2023　Elsevier　Inc.